Polyarylene sulfide resin composition and method for preparing the same

ABSTRACT

PCT No. PCT/JP91/01090 Sec. 371 Date Mar. 30, 1992 Sec. 102(e) Date Mar. 30, 1992 PCT Filed Aug. 15, 1991 PCT Pub. No. WO92/03508 PCT Pub. Date Mar. 5, 1992.A polyarylene sulfide resin composition useful for molding articles is obtained by mixing and melt kneading a polyarylene sulfide resin, a polyamide resin, a silane compound and either water or an alcohol having a boiling point of at least 100 DEG C.

FIELD OF THE INVENTION

The present invention relates to an improved polyarylene sulfide resincomposition and a method of preparing the same.

More particularly, the present invention relates to a polyarylenesulfide resin composition having excellent impact resistance and heatresistance and which is produced by blending specific amounts ofalkoxysilane compound, water and the like to a resin componentcomprising a polyarylene sulfide resin and a polyamide resin, and heatmelting and kneading the resultant blend, and to the method of preparingsame.

BACKGROUND OF THE INVENTION

Recently, a thermoplastic resin having high heat and chemical resistanceand excellent flame retardance has been demanded as the material ofconstruction for the components of electrical or electronic appliances,automobile devices or chemical instruments.

Polyarylene sulfide resin, represented by polyphenylene sulfide, is oneof the resins satisfying this demand and is inexpensive relative to theexcellent properties thereof, such that the demand for polyarylenesulfide resin has increased. However, polyarylene sulfide resin hascritical disadvantages in that it is inferior to other engineeringplastics such as nylon, polycarbonate, polyacetal, polybutyleneterephthalate, and the like, because polyarylene sulfide resin has poorductility and is therefore brittle.

As a means for overcoming these problems, it is known that blending afibrous reinforcement material such as glass fiber or carbon fiber andother fillers improves the properties of polyarylene sulfide resin suchas strength, rigidity, toughness, heat resistance and the like. However,even by blending such reinforcement materials with polyarylene sulfideresin, the resin still has poor toughness compared with the engineeringplastics described above, and the application polyarylene sulfide resinfor a great number of uses may be limited in some cases, even though theresin has excellent chemical resistance, heat resistance andnonflammability.

The present inventors have made thorough investigations of polyarylenesulfide resin compositions having high toughness and impact resistanceand the method for preparing the same, and examined a reactive substancecapable of reacting with both polyarylene sulfide resin and polyamideresin. Consequently, it has been found that a silane compound having aalkoxysilane group within the molecule thereof provides an improvementin impact strength of the blend. The inventors have applied for patentsas Japanese Patent Laid-open Nos. 320140/1989, 44140/1990 and110839/1990 on such composition and the method for preparing same. Theimproved blend realizes good toughness and impact strength, but thephysical properties thereof may vary occasionally. Accordinglyimprovement has been desired.

SUMMARY OF THE INVENTION

The present inventors have found that to stably produce a polyarylenesulfide resin composition with still more improved toughness and impactstrength, the presence of water and the like is influential. Accordinglyblending an alkoxysilane compound and a specific amount of water oralcohols with a boiling point of 100° C. or more, with a blend ofpolyarylene sulfide resin and polyamide resin, and processing andkneading the resultant blend at a specific temperature for a specificperiod of time, a molding material with remarkably high toughness andutility can be produced in a stable fashion. The present inventiontherefore relates to a method of preparing a polyarylene sulfide resincomposition, comprising mixing (C) 0.01 to 5 parts by weight of at leastone silane compound selected from the group consisting ofvinylalkoxysilane, epoxyalkoxysilane, aminoalkoxysilane,mercaptoalkoxysilane and allylalkoxysilane, and (D) 0.03 to 5 moles permole of the component (C) of water, or at least one alcohol selectedfrom alcohols with a boiling point of 100° C. or more, or a mixturethereof, with 100 parts by weight of a resin component comprising (A) 97to 20 parts by weight of a polyarylene sulfide resin and (B) 3 to 80parts by weight of a polyamide resin, and processing the resultantmixture by heat melting and kneading in the presence of at least theabove four components for 30 seconds or more, and relates to a resincomposition produced according to the method for preparing the same.

DETAILED DESCRIPTION OF THE INVENTION

The polyarylene sulfide resin as the component (A) to be used in thepresent invention is constituted mainly of repeating units -(Ar-S)-(provided that Ar is arylene group).

As the arylene group, there can be used p-phenylene group, m-phenylenegroup, o-phenylene group, substituted phenylene groups (provided thatthe substituent is an alkyl group, preferably an alkyl group of C₁ to C₅or a phenylene group), p,p'-diphenylene sulfone group, p,p'-biphenylenegroup, p,p'-diphenylene ether group, p,p'-diphenylene carbonyl group,naphthalene group and the like.

In this invention, there can be used a polymer employing an identicalrepeating unit among the arylene sulfide group constituted of thearylene groups described above, namely a homopolymer. A copolymercontaining different repeating units may be preferable in some cases.

As the homopolymer, a substantially linear one with p-phenylene sulfidegroup as the repeating unit and in which p-phenylene group is employedas the arylene group, is perferably used.

As the copolymer, there can be used a combination of two or moredifferent arylene sulfide groups comprising the arylene group describedabove, but in particular a combination of p-phenylene sulfide groups inthe main and containing m-phenylene sulfide groups is preferably used.Among copolymers, substantially linear ones containing 60 mole % ormore, more preferably 70 mole % or more of p-phenylene sulfide groups,are suitable from the standpoint of physical properties such as heatresistance, moldability and mechanical properties.

Further, copolymers containing 5 to 40 mole %, in particular 10 to 25mole % of m-phenylene sulfide group are preferable as the copolymer.

In this invention, those copolymers containing component-repeating unitsin block form (for example, those described in Japanese Patent Laid-openNo. 14228/1986) rather than in a random form can be used favorably,because of good processability and excellent heat resistance andmechanical properties thereof.

The polyarylene sulfide resin as component (A) to be used in the presentinvention, there can be employed a polymer with the moldingprocessability improved by crosslinking the polymer described aboveoxidatively or thermally whereby its melt viscosity is increased. Therecan also be used a polymer having a substantially linear structure,obtained by polycondensation of principally bifunctional monomers. Inmany cases, the latter polymer having a substantially linear structureis superior with respect to the physical properties of the moldedarticles thus obtained.

As the polyarylene sulfide resin of the present invention, there canpreferably be used, other than the polymers described above, a resinprepared by blending with the linear polymer described above acrosslinked polyarylene sulfide resin prepared by using and polymerizingmonomers with three or more functional groups in combination as a partof the monomer.

The polyamide resin useful as component (B) of the present inventionincludes various known polyamide resins. These include for example,polyamide resins obtained by polycondensing dicarboxylic acid such asoxalic acid, adipic acid, suberic acid, sebacic acid, terephthalic acid,isophthalic acid, and 1,4-cyclohexyl dicarboxylic acid, with diaminesuch as ethylene diamine, pentamethylene diamine, hexamethylene diamine,decamethylene diamine, 1,4-cyclohexyl diamine and m-xylylene diamine;polyamide resins obtained by polymerizing cyclic lactam such ascaprolactam and lauric lactam; polyamide resins obtained bycopolymerizing cyclic lactam and the salts of dicarboxylic acid anddiamine or the like. Among these polyamide resins, nylon 6, nylon 66,nylon 12, the copolymers thereof and the like are illustratedpreferably.

Also, polyamide elastomer resins can be used as the polyamide resin asthe component (B). Polyamide elastomer resins are polyamide blockcopolymers having a bending modulus of 10,000 kgf/cm² or less (relativehumidity of 50% and 23° C.) composed of polyamide hard segments bondedwith other soft segments. As the soft segments of such elastomer,polyalkylene oxide (the alkylene group having 2 to 6 carbon atoms) is arepresentative example. A great number of reports have been made aboutthe synthesis of such polyamide elastomers, and the synthesis iscommonly carried out in two stages i.e., the production of nylonoligomer and the polymerization thereof by esterification. The polyamidecomponent as the hard segment herein includes the polyamides such aspolyamide 6, polyamide 66, polyamide 6,12, polyamide 11, polyamide 12and the like; the polyether component as the soft segment includespolyoxyethylene glycol, polyoxypropylene glycol, polyoxytetramethyleneglycol and the like.

Furthermore, the polyamide resin as the component (B) is not limited toone type, as two or more types may be used in combination in order tocontrol the physical properties.

In accordance with the present invention, the mixing amount of polyamideresin (B) is 3 to 80% by weight to the total amount of the components(A) and (B). If the component (B) is much less, a lower effect isobtained with respect to toughness improvement; if too much, theadvantage of the polyarylene sulfide resin (A) is deteriorated.

The present invention is characterized by adding and mixing thealkoxysilane compound (C) along with the above resin components.

The alkoxysilane (C) to be used in the present invention is selectedfrom one or more of vinylalkoxysilane, epoxyalkoxysilane,aminoalkoxysilane, mercaptoalkoxysilane, allylalkoxysilane, etc.

Examples of vinylalkoxysilane include vinyltriethoxysilane,vinyltrimethoxysilane, and vinyltris(β-methoxyethoxy)silane, etc.

Examples of epoxyalkoxysilane include γ-glycidoxypropyltrimethoxysilane,β-(3,4-epoxycyclohexyl)ethyltrimethoxysilane, andγ-glycidoxypropyltriethoxysilane, etc.

Examples of aminoalkoxysilane include γ-aminopropyltrimethoxysilane,γ-aminopropyltriethoxysilane, γ-aminopropyldimethoxysilane,γ-aminopropylmethyldiethoxysilane,N-(β-aminoethyl)-γ-aminopropyltrimethoxysilane,N-phenyl-γ-aminopropyltrimethoxysilane, etc.

Examples of mercaptoalkoxysilane includeγ-mercaptopropyltrimethoxysilane, γ-mercaptopropyltriethoxysilane, etc.

Examples of allylalkoxysilane includeγ-diallylaminopropyltrimethoxysilane,γ-allylaminopropyltrimethoxysilane, γ-allylthiopropylltrimethoxysilane,etc..

The amount of the alkoxysilane compound to be used as the component (C)is 0.01 to 5 parts by weight, preferably 0.1 to 3 parts by weight to 100parts by weight of the total amount of polyarylene sulfide resin[component (A)] and polyamide resin [component (B)].

The amount of alkoxysilane compound to be added varies depending on thetype thereof and the use of the objective compositions. If too little isused, a lower effect is obtained on toughness improvement; if too much,the melt viscosity increased excessively causing disadvantages duringmold processing.

The present invention is characterized in that a controlled amount ofwater or alcohols with a boiling point of 100° C. or more, as component(D), are added along with components (A), (B) and (C), and the mixtureheat melted and kneaded. Unfavorably, alcohols with a boiling point of100° C. or less vaporize during the heat melting process, so theireffect may not be sufficiently exhibited. The alcohols with a boilingpoint of 100° C. or more belonging to component (D) to be used in thepresent invention, include for example isobutyl alcohol, isopentylalcohol, cyclohexanol, benzyl alcohol, ethylene glycol, propyleneglycol, butanediol, pentanediol, neopentyl glycol, hexanediol,octanediol, decanediol, glycerine, diethylene glycol, triethyleneglycol, pentaerythritol, clohexanedimethanol, hydroquinone,N-ethyl-2,2'-iminodiethanol, N-butyl-2,2'-iminodiethanol, 2-butyl1,4-diol, 2-butene 1,4-diol, bisphenol A,2,2'-bis(4-hydroxyethoxyphenyl)propane, xylene glycol, etc..

It is required to regulate the amount of the component (D) to be usedwithin a range of 0.03 to 5 mole, preferably 0.03 to 3 mole, per onemole of the component (C). The amount of the component (D) to be addedvaries, depending on the type, the preparative method of thecompositions and the objective physical properties of the compositions.Problems may arise concerning the stable production of compositions withgood toughness if the amount of component (D) added is too small;whereas disadvantages may be caused by the occurrence of bleedout on thesurface of molded articles if the amount is too much. Further, thepreferable amount of the component (D) to be used will vary depending onthe mode as to how the component is added and blended. In other words,in the case in which component (D) is preliminarily added to thealkoxysilane compound (C) and then kneaded with other components, arelatively small amount is generally preferable within the rangedescribed above. In the case in which component (D) is added and blendedin the state of being adsorbed onto other components (or beinghumidified), a relatively greater amount may be appropriate. Regardingthe method as to how to add component (D), component (D) may be added toany one of the components (A), (B), and (C), and the component (E) insome cases. It is particularly preferable to preliminarily add component(D) to the alkoxysilane compound (C). Also, in case of using alcoholswith a boiling point of 100° C. or more as the component (D), it hasbeen observed that alcohols with two or more hydroxyl groups within theindividual molecule rather than those with one hydroxyl group within theindividual molecules tend to exert the beneficial effects using asmaller amount thereof.

Other than the components described above, the composition of thepresent invention can be blended with an inorganic filler, as thecomponent (E). Preferably, such filler (E) is blended in order toproduce molded articles having excellent properties such as mechanicalstrength, heat resistance, dimensional stability, electrical propertiesand the like. Fibrous, powdery and flaky fillers are used as the filler(E), depending on the object.

As fibrous fillers, there are included inorganic fibrous materials suchas glass fiber, asbestos fiber, carbon fiber, silica fiber,silica/alumina fiber, zirconia fiber, boron nitride fiber, siliconnitride fiber, boron fiber and potassium titanate fiber, and fibers ofmetals including stainless steel, aluminum, titanium, copper or brass.Particularly representative fibrous fillers are glass fiber or carbonfiber. Further, organic fibrous materials with high melting points mayalso be used, including polyamides, fluororesins, alkali resins and thelike.

Alternatively, the powdery filler includes carbon black, silica, quartzpowder, glass bead, glass powder, silicates such as calcium silicate,aluminum silicate, kaolin, talc, clay, diastomaceous earth andwollastonite, metal oxides such as iron oxide, titanium oxide andalumina; metal carbonates such as calcium carbonate and magnesiumcarbonate; metal sulfates such as calcium sulfate and barium sulfate;silicon carbide, silicon nitride, boron nitride and various metalpowders.

The flaky filler includes mica, glass flake and various metal foils.

These inorganic fillers may be used alone or in combination of two ormore thereof. The concurrent use of a fibrous filler, in particularglass or carbon fiber, with a powdery or flaky filler is preferable as acombination with respect to the provision of mechanical strength,dimensional precision and electrical properties.

The amount of inorganic filler to be added is 400 parts by weight orless per 100 parts by weight of the total amount of the resin components(A) and (B). If the amount of filler exceeds this, the processabilityduring molding and toughness are deteriorated unfavorably. It isspecifically preferable to add 250 parts by weight or less of filler per100 parts by weight of (A) and (B).

To the composition of the present invention herein can be added as asupplement a small amount of other thermoplastic resins within a rangewithout damaging the objects of the present invention, in addition to apolyarylene sulfide resin and a polyamide resin. The thermoplasticresins herein used may be any thermoplastic resin stable at a hightemperature approximately of the melting temperature of a polyarylenesulfide resin.

For example, there are illustrated olefin polymer, aromatic polyesterpolymer comprising aromatic dicarboxylic acid such as polyethyleneterephthalate, polybutylene terephthalate, complete aromatic polyester,etc. and diol or oxycarboxylic acid, polycarbonate, ABS, polyphenyleneoxide, polyalkylacrylate, polyacetal, polysulfone, polyether sulfone,polyether imide, polyether ketone, fluororesin, etc.. Furthermore, thesethermoplastic resins may be used in combination of two or more thereof.Among them, ethylene copolymer or its graft copolymer as polyolefinpolymer, for example, copolymer of ethylene and α,β-unsaturated fattyacid or alkyl ester or glycidyl ester thereof, and the graft copolymerproduced by further grafting vinyl polymer with the copolymer, and thelike, are specifically preferable as an auxiliary component.

The composition of the present invention can be prepared by knownmethods, but it is required to mix and knead simultaneously at least thefour components (A), (B), (C) and (D) at the heat melted state thereoffor 30 seconds or more. Generally, the component (D) is preliminarilyadded to the component (C), and the resulting mixture is blended withthe components (A) and (B), and (E) if necessary, which is thenpreliminarily mixed uniformly with a mixer such as a tumbler or aHenschel mixer. The resultant mixture is then fed to a uniaxial orbiaxial extruder for heat melting and kneading, to be prepared aspellets. The components (A), (B), (C) and (D) may be directly mixed,without preliminarily adding the component (D) to the component (C); orthe component (D) may be preliminarily adsorbed onto the component (A)or (B), which is then mixed with the component (C). In this latter case,the tendency is that a greater amount of component (D) is needed,compared with the amount of component (D) in case in which component (D)is preliminarily added to component (C). Furthermore, the form of thecomponents (A) and (B) may be pellets, but a part of the component (A)or (B) or its entirety is preferably made into powder. Preferably, amixture of (C) and (D) is added to the part of the powder, or (C) and(D) are added separately to the part of the powder. The resultantmixture is uniformly mixed once with a blender, which is then uniformlymixed with the remaining components for the process of heat melting andkneading. Also, the component (E) may be added during or after theprocess of heat melting and kneading.

The temperature for the process of heat melting and kneading is higherby 5° C. to 100° C. than the melting point of the resin component, andis preferably higher by 10° C. to 60° C. than the resin melting point.At temperatures too high, the degradation of the resin and abnormalreactions may unfavorably result. Further, the period of time for heatmelting and kneading varies depending on the temperature of theprocessing and the types and amounts of components (C) and (D) added.The time for heat melting and kneading is at least 30 seconds or moreand 15 minutes or less, and preferably 1 to 10 minutes.

The detailed mechanism of the actions and effects between thealkoxysilane compound component (C) and component (D) of the presentinvention has not yet thoroughly elucidated, but it is believed that thepolyarylene sulfide molecule and polyamide molecule are efficientlybonded together via the presence of component (D), to improve thecompatibility between the components (A) and (B). This is confirmed byelectron microscopic observation of the cross section of a moldedarticle from the composition. That is, in case of components (A) and (B)solely, the dispersion components are present as coarse particles (forexample, 10 μ or less). According to the method of the presentinvention, it is observed that the dispersion components are indispersion as extremely uniform and fine particles (at most 3μ or less,and generally 1μ or less).

Furthermore, there may be added antioxidants, heat stabilizers,lubricants, nucleating agents, ultraviolet absorbers, colorants, moldrelease agents, and other common additives, within a range withoutdeviating from the objects of the present invention.

These additives may be added and blended, simultaneously with orseparately from the process of heat melting and kneading. Effects of theInvention

The polyarylene sulfide resin composition of the present invention hasthe following effects;

(1) Molded articles with good mechanical properties such as tensileelongation, impact strength, etc. are produced in a stable fashion;

(2) The balance between the heat resistance and the mechanicalproperties is maintained at a higher degree.

EXAMPLES

The present invention will now be explained more concretely in thefollowing examples, but the present invention is not intended to belimited solely to the embodiments shown therein.

EXAMPLES 1 TO 3, COMPARATIVE EXAMPLES 1 TO 3

Water was added to γ-aminopropyltriethoxysilane at the ratios shown inTable 1, with subsequent blending of polyphenylene sulfide polymer (amelting point of 285° C., a melt viscosity of 500 poise as measured at310° C. and a shear rate of 1200 sec⁻¹), and nylon 66, and in some casesglass fiber (chopped strand of 10 μm diameter and 3 mm in length), atthe ratios shown in Table 1, which were then preliminarily mixedtogether for five minutes. The resultant mixture was heat melted andkneaded in an extruder at 310° C. (residence time of about 3 minutes) toproduce pellets of polyphenylene sulfide resin composition.

Then, 10 ASTM test pieces were individually molded at the conditions ofa cylinder temperature of 310° C. and a mold temperature of 150° C., tocarry out tensile test, impact test, and thermal deformation test.

The results are shown in Table 1. Concerning tensile elongation and Izodimpact strength, the maximum and minimum and mean values of samples areshown in Table 1. (Change in the amount of the component (C).)

EXAMPLES 4 TO 7, COMPARATIVE EXAMPLES 4 TO 7

As in the above Examples and Comparative Examples, using polyphenylenesulfide polymer and nylon 66 at the blend ratios shown in Table 2(change in (A): (B)), tests were performed as in Examples 2 and 3, andComparative Examples 2 and 3. The results are shown in Table 2.

EXAMPLES 8 TO 11

As in the above Examples and Comparative Examples, using polyphenylenesulfide polymer and nylon 66 at the blend ratios shown in Table 3(change in the amount of (D)), tests were performed as in Examples 2 and3, and Comparative Examples 2 and 3. The results are shown in Table 3.

EXAMPLES 12 TO 15, COMPARATIVE EXAMPLES 8 TO 11

Replacing the nylon 66 in the Examples 2 and 3 and Comparative Examples2 and 3 with nylon 6 or nylon 12, tests were performed at the blendratios shown in Table 4, as in Examples 2 and 3, and ComparativeExamples 2 and 3. The results are shown in Table 4.

EXAMPLES 16 TO 19, COMPARATIVE EXAMPLES 12 TO 15

Replacing the γ-aminopropyltriethoxysilane in Example 2 and ComparativeExample 2 with γ-glycidoxypropyltrimethoxysilane,γ-mercaptopropyltrimethoxysilane, vinyltrimethoxysilane, andγ-diallylaminopropyltrimethoxysilane, tests were performed at the blendratios shown in Table 5, as in Example 2 and Comparative Example 2. Theresults are shown in Table 5.

EXAMPLES 20 TO 23

Replacing the water in Example 2 and Comparative Example 2 with benzylalcohol, ethylene glycol, butanediol and glycerin, tests were performedat the blend ratios shown in Table 6, as in Example 2 and ComparativeExample 2. The results are shown in Table 6.

EXAMPLES 24 AND 25

Water was preliminarily added to or was made to humidify the powderypolyphenylene sulfide resin or nylon 66 described above at the ratiosshown in Table 7, and blending was effected along with other componentsat the ratios shown in Table 7, which was then preliminarily mixedtogether with a Henschel mixer for five minutes. After the preliminarymixing, tests were performed as in Example 2. The results are shown inTable 7.

                                      TABLE 1                                     __________________________________________________________________________                        Comp. Ex. 1                                                                          Ex. 1                                                                              Comp. Ex. 2                                                                          Ex. 2                                                                              Comp. Ex. 3                                                                          Ex. 3                      __________________________________________________________________________    Blend ratio                                                                   (A) polyphenylene sulfide resin (pts.                                                             60     60   60     60   60     60                         by wt.)                                                                       (B) nylon 66 resin (pts.                                                                          40     40   40     40   40     40                         by wt.)                                                                       (C) γ-aminopropyltriethoxysilane (pts.                                                        0.5    0.5                                                                                2.0    2.0                                                                                2.0    2.0                      by wt.)                                                                       (D) water (in mole per one mole of (C))                                                           --        0.05                                                                            --        0.05                                                                            --        0.05                    (E) glass fiber (pts. by wt)                                                                      --     --   --     --   67     67                         Physical properties of compositions                                           tensile strength (kgf/cm.sup.2)                                                                   778    782  845    852  2340   2350                       tensile elongation                                                                           mean 30     34   48     52     5.7    6.1                      (%)            maximum                                                                            36     38   57     58     6.4    6.6                                     minimum                                                                            18     31   21     46     3.6     5.7                     Izod impact strength notched                                                                 mean   3.4    3.6                                                                                5.0    5.3                                                                                12.4   12.9                     (kgcm/cm)      maximum                                                                              3.8    3.9                                                                                5.7    5.8                                                                                13.9   14.0                                    minimum                                                                              2.5    3.3                                                                                2.7    4.8                                                                                7.8    12.6                     Izod impact strength unnotched                                                               mean 48     53   80     85   52     57                         (kgcm/cm)      maximum                                                                            55     57   94     95   59     61                                        minimum                                                                            30     47   37     77   34     54                         thermal deformation temperature [°C.],                                                     110    110  108    108  254    254                        18.6 kg load                                                                  __________________________________________________________________________

                                      TABLE 2                                     __________________________________________________________________________                        Comp.    Comp.    Comp.    Comp.                                              Ex. 4                                                                             Ex. 4                                                                              Ex. 5                                                                             Ex. 5                                                                              Ex. 6                                                                             Ex. 6                                                                              Ex. 7                                                                             Ex. 7                      __________________________________________________________________________    Blend ratio                                                                   (A) polyphenylene sulfide resin (pts.                                                             80  80   40  40   80  80   40  40                         by wt.)                                                                       (B) nylon 66 resin (pts. by wt.)                                                                  20  20   60  60   20  20   60  60                         (C) γ-aminopropyltriethoxysilane (pts.                                                        2.0                                                                               2.0                                                                                2.0                                                                               2.0                                                                                2.0                                                                               2.0                                                                                2.0                                                                               2.0                      by wt.)                                                                       (D) water (in mole per one mole of (C))                                                           --     0.05                                                                            --     0.05                                                                            --     0.05                                                                            --     0.05                    (E) glass fiber (pts. by wt)                                                                      --  --   --  --   67  67   67  67                         Physical properties of compositions                                           tensile strength (kgf/cm.sup.2)                                                                   718 722  835 842  2010                                                                              2030 2335                                                                              2350                       tensile elongation                                                                           mean 32  35   60  64     4.0                                                                               4.2                                                                                6.9                                                                               7.2                      (%)            maximum                                                                            37  39   69  70     4.7                                                                               4.8                                                                                8.0                                                                               8.1                                     minimum                                                                            21  32   32  57     2.4                                                                               3.8                                                                                3.1                                                                               6.5                      Izod impact strength notched                                                                 mean   4.0                                                                               4.3                                                                                5.6                                                                               5.9                                                                                11.0                                                                              11.2                                                                               12.7                                                                              13.2                     (kgcm/cm)      maximum                                                                              4.6                                                                               4.7                                                                                6.5                                                                               6.6                                                                                12.2                                                                              12.3                                                                               14.1                                                                              14.3                                    minimum                                                                              2.5                                                                               3.9                                                                                3.0                                                                               5.1                                                                                6.8                                                                               10.5                                                                               8.2                                                                               12.0                     Izod impact strength unnotched                                                               mean 66  69   95  98   41  45   58  61                         (kgcm/cm)      maximum                                                                            77  78   110 114  47  49   65  66                                        minimum                                                                            35  62   47  88   31  42   39  57                         thermal deformation temperature [°C.],                                                     114 114  95  95   256 256  251 251                        18.6 kg load                                                                  __________________________________________________________________________

                                      TABLE 3                                     __________________________________________________________________________                        Comp. Ex. 2                                                                          Ex. 2                                                                              Ex. 8                                                                             Ex. 9                                                                             Ex. 10                                                                             Comp. Ex. 3                                                                          Ex.                       __________________________________________________________________________                                                        11                        Blend ratio                                                                   (A) polyphenylene sulfide resin (pts.                                                             60     60   60  60  60   60     60                        by wt.)                                                                       (B) nylon 66 resin (pts. by wt.)                                                                  40     40   40  40  40   40     40                        (C) γ-aminopropyltriethoxysilane (pts.                                                        2.0    2.0                                                                                2.0                                                                               2.0                                                                               2.0                                                                                2.0    2.0                     by wt.)                                                                       (D) water (in mole per one mole of (C))                                                           --        0.05                                                                              0.5                                                                              1   3   --      3                        (E) glass fiber (pts. by wt)                                                                      --     --   --  --  --   67     67                        Physical properties of compositions                                           tensile strength (kgf/cm.sup.2)                                                                   845    852  852 851 848  2340   2345                      tensile elongation                                                                           mean 48     52   52  54  56     5.7    6.3                     (%)            maximum                                                                            57     58   58  59  61      6.4   6.7                                    minimum                                                                            21     46   46  50  52     3.6    5.9                     Izod impact strength notched                                                                 mean   5.0    5.3                                                                                5.3                                                                               5.5                                                                               5.6                                                                                12.4   13.0                    (kgcm/cm)      maximum                                                                              5.7    5.8                                                                                5.7                                                                               5.8                                                                               6.1                                                                                13.9   13.5                                   minimum                                                                              2.7    4.8                                                                                4.9                                                                               5.0                                                                               5.2                                                                                7.8    12.7                    Izod impact strength unnotched                                                               mean 80     85   85  86  88   52     59                        (kgcm/cm)      maximum                                                                            94     95   88  90  92   59     63                                       minimum                                                                            37     77   81  81  83   34     55                        thermal deformation temperature [°C.],                                                     108    108  108 108 107  254    254                       18.6 kg load                                                                  __________________________________________________________________________

                                      TABLE 4                                     __________________________________________________________________________                        Comp.    Comp.    Comp.    Comp.                                              Ex. 8                                                                             Ex. 12                                                                             Ex. 9                                                                             Ex. 13                                                                             Ex. 10                                                                            Ex. 14                                                                             Ex. 11                                                                            Ex. 15                     __________________________________________________________________________    Blend ratio                                                                   (A) polyphenylene sulfide resin (pts.                                                             60  60   60  60   60  60   60  60                         by wt.)                                                                       (B)                                                                              nylon 6 resin (pts. by wt.)                                                                    40  40   --  --   40  40   --  --                            nylon 12 resin (pts. by wt.)                                                                   --  --   40  40   --  --   40  40                         (C) γ-aminopropyltriethoxysilane (pts.                                                       2   2    2   2    2   2    2   2                         by wt.)                                                                       (D) water (in mole per one mole of (C))                                                           --     0.05                                                                            --     0.05                                                                            --     0.05                                                                            --     0.05                    (E) glass fiber (pts. by wt)                                                                      --  --   --  --   67  67   67  67                         Physical properties of compositions                                           tensile strength (kgf/cm.sup.2)                                                                   825 834  705 710  2100                                                                              2120 2000                                                                              2000                       tensile elongation                                                                           mean 60  64   45  50     8.7                                                                               9.2                                                                                7.3                                                                               7.8                      (%)            maximum                                                                            69  70   56  58     9.4                                                                               9.8                                                                                8.5                                                                               8.7                                     minimum                                                                            35  56   20  44     5.6                                                                               8.5                                                                                3.6                                                                               7.0                      Izod impact strength notched                                                                 mean   7.2                                                                               7.6                                                                                5.1                                                                               5.5                                                                                13.2                                                                              13.6                                                                               12.0                                                                              12.5                     (kgcm/cm)      maximum                                                                              8.0                                                                               8.3                                                                                5.9                                                                               6.1                                                                                14.5                                                                              14.7                                                                               13.3                                                                              13.5                                    minimum                                                                              3.9                                                                               7.0                                                                                2.8                                                                               5.0                                                                                8.9                                                                               12.4                                                                               7.9                                                                               11.6                     Izod impact strength unnotched                                                               mean 98  110  70  76   65  69   51  56                         (kgcm/cm)      maximum                                                                            113 121  83  85   73  75   59  61                                        minimum                                                                            51  101  40  66   46  61   35  47                         thermal deformation temperature [°C.],                                                     107 107  80  80   247 247  236 236                        18.6 kg load                                                                  __________________________________________________________________________

                                      TABLE 5                                     __________________________________________________________________________                        Comp.    Comp.    Comp.    Comp.                                              Ex. 12                                                                            Ex. 16                                                                             Ex. 13                                                                            Ex. 17                                                                             Ex. 14                                                                            Ex. 18                                                                             Ex. 15                                                                            Ex. 19                     __________________________________________________________________________    Blend ratio                                                                   (A) polyphenylene sulfide resin (pts.                                                             60  60   60  60   60  60   60  60                         by wt.)                                                                       (B) nylon 66 resin (pts. by wt.)                                                                  40  40   40  40   40  40   40  40                         (C)                                                                              γ-glycidoxypropyltrimethoxysilane                                                         2   2   --  --   --  --   --  --                            (pts. by wt.)                                                                 γ-mercaptopropyltrimethoxysilane                                                         --  --    2   2   --  --   --  --                            (pts. by wt.)                                                                 vinyltrimethoxysilane (pts. by wt.)                                                            --  --   --  --    2   2   --  --                            γ-diallylaminopropyltrimethoxy                                                           --  --   --  --   --  --    2   2                            silane (pts. by wt.)                                                       (D) water (in mole per one mole of (C))                                                           --     0.05                                                                            --     0.05                                                                            --     0.05                                                                            --     0.05                    (E) glass fiber (pts. by wt)                                                                      --  --   --  --   --  --   --  --                         Physical properties of compositions                                           tensile strength (kgf/cm.sup.2)                                                                   865 875  810 820  825 835  840 845                        tensile elongation                                                                           mean 54  58   42  45   46  49   47  50                         (%)            maximum                                                                            61  64   49  51   54  55   55  57                                        minimum                                                                            30  52   22  38   27  41   29  44                         Izod impact strength notched                                                                 mean   6.0                                                                               6.3                                                                                4.5                                                                               4.8                                                                                4.8                                                                               5.2                                                                                4.9                                                                               5.2                      (kgcm/cm)      maximum                                                                              6.8                                                                               7.2                                                                                5.3                                                                               5.4                                                                                5.7                                                                               5.8                                                                                5.8                                                                               5.8                                     minimum                                                                              3.5                                                                               5.5                                                                                2.5                                                                               4.0                                                                                2.9                                                                               4.5                                                                                3.1                                                                               4.4                      Izod impact strength unnotched                                                               mean 95  100  70  74   75  79   78  82                         (kgcm/cm)      maximum                                                                            112 114  83  85   88  94   89  98                                        minimum                                                                            46  88   38  66   43  68   44  70                         thermal deformation temperature [°C.],                                                     107 107  109 109  108 108  108 108                        18.6 kg load                                                                  __________________________________________________________________________

                                      TABLE 6                                     __________________________________________________________________________                        Comp. Ex. 2                                                                          Ex. 20                                                                            Ex. 21                                                                            Ex. 22                                                                            Ex. 23                                 __________________________________________________________________________    Blend ratio                                                                   (A) polyphenylene sulfide resin (parts                                                            60     60  60  60  60                                     by wt.)                                                                       (B) nylon 66 resin (pts. by wt.)                                                                  40     40  40  40  40                                     (C) γ-aminopropyltriethoxysilane (pts.                                                       2      2   2   2   2                                     by wt.)                                                                       (D)                                                                              benzylalcohol (in mole per one                                                                 --       1.0                                                                             --  --  --                                        mole of (C))                                                                  ethylene glycol (in mole per one                                                               --     --    1.0                                                                             --  --                                        mole of (C))                                                                  butanediol (in mole to one mole                                                                --     --  --    1.0                                                                             --                                        of (C))                                                                       glycerine (in mole per one                                                                     --     --  --  --    1.0                                     mole of (C))                                                               (E) glass fiber (pts. by wt)                                                                      --     --  --  --  --                                     Physical properties of compositions                                           tensile strength (kgf/cm.sup.2)                                                                   845    850 853 853 854                                    tensile elongation                                                                           mean 48     51  53  52  54                                     (%)            maximum                                                                            57     57  59  60  59                                                    minimum                                                                            21     40  48  47  50                                     Izod impact strength notched                                                                 mean   5.0    5.1                                                                               5.4                                                                               5.4                                                                               5.6                                  (kgcm/cm)      maximum                                                                              5.7    5.6                                                                               5.8                                                                               5.9                                                                               6.0                                                 minimum                                                                              2.7    4.1                                                                               4.8                                                                               4.9                                                                               5.1                                  Izod impact strength unnotched                                                               mean 80     83  85  85  86                                     (kgcm/cm)      maximum                                                                            94     94  96  97  100                                                   minimum                                                                            37     60  78  77  80                                     thermal deformation temperature [°C.],                                                     108    108 108 108 108                                    18.6 kg load                                                                  __________________________________________________________________________

                                      TABLE 7                                     __________________________________________________________________________                        Comp. Ex. 2                                                                          Ex. 24                                                                            Ex. 25                                                                            Ex. 3                                      __________________________________________________________________________    Blend ratio                                                                   (A) polyphenylene sulfide resin (parts                                                            60     60  60  60                                         by weight)                                                                    (B) nylon 66 resin (pts. by wt.)                                                                  40     40  40  40                                         (C) γ-aminopropyltriethoxysilane (pts.                                                       2      2   2   2                                         by wt.)                                                                       (D)                                                                              water added to (A) (in mole per                                                                --       0.5                                                                             --  --                                            one mole of (C))                                                              water added to (B) (in mole per                                                                --     --    0.5                                                                             --                                            one mole of (C))                                                              water added to (C) (in mole per                                                                --     --  --    0.5                                         one mole of (C))                                                           (E) glass fiber (pts. by wt)                                                                      --     --  --  --                                         Physical properties of compositions                                           tensile strength (kgf/cm.sup.2)                                                                   845    851 852 852                                        tensile elongation                                                                           mean 48     50  51  52                                         (%)            maximum                                                                            57     57  59  58                                                        minimum                                                                            21     40  45  46                                         Izod impact strength notched                                                                 mean   5.0    5.2                                                                               5.3                                                                               5.3                                      (kgcm/cm)      maximum                                                                              5.7    5.8                                                                               5.7                                                                               5.7                                                     minimum                                                                              2.7    4.1                                                                               4.7                                                                               4.9                                      Izod impact strength unnotched                                                               mean 80     85  84  85                                         (kgcm/cm)      maximum                                                                            94     91  90  88                                                        minimum                                                                            37     74  80  81                                         thermal deformation temperature [°C.],                                                     108    108 108 108                                        18.6 kg load                                                                  __________________________________________________________________________

We claim:
 1. A method of preparing a polyarylene sulfide resincomposition, comprising; forming a mixture of the followingcomponents:(A) 97 to 20 parts by weight of a polyarylene sulfide resinand (B) 3 to 80 parts by weight of a polyamide resin, with (C) 0.01 to 5parts by weight of at least one silane compound selected from the groupconsisting of vinylalkoxysilane, epoxyalkoxysilane, aminoalkoxysilane,mercaptoalkoxysilane and allylalkoxysilane, and (D) 0.03 to 5 moles permole of said silane compound (C) of water or at least one alcohol havinga boiling point of 100° C. or more, and heat melting and kneading saidmixture for 30 seconds or more.
 2. The method of claim 1 wherein saidcomponent (D) is said at least one alcohol each having at least twohydroxyl groups.
 3. The method of claim 1 wherein said polyarylenesulfide resin (A) comprises polyphenylene sulfide.
 4. The method ofclaim 3 wherein said polyphenylene sulfide comprises a homopolymercomposed of p-phenylene sulfide groups.
 5. The method of claim 3 whereinsaid polyphenylene sulfide comprises a copolymer composed p-phenylenesulfide groups and m-phenylene sulfide groups.
 6. The method of claim 5wherein said copolymer comprises 5 to 40 mole % of said m-phenylenesulfide groups and 60 to 95 mole % of said p-phenylene sulfide groups.7. The method of claim 1 wherein said polyamide resin (B) is selectedfrom nylon 6, nylon 66, nylon 12 and copolymers thereof.
 8. The methodof claim 1 wherein said component (D) is water.
 9. The method of claim 1wherein said mixture is formed by mixing component (D) with said onesilane compound (C) and adding the mixture of (C) and (D) to a mixtureof said polyarylene sulfide resin (A) and said polyamide resin (B) priorto said heat melting and kneading.
 10. The method of claim 1 whereinsaid mixture is formed by mixing said component (D) with saidpolyarylene sulfide resin (A), said polyamide resin (B) or a mixture of(A) and (B) prior to mixing with said component (C).
 11. The method ofclaim 10 wherein said component (D) is water.
 12. The method of claim 5further mixing (E) 1 to 400 parts by weight of at least one filler withsaid mixture.
 13. The method of claim 12 wherein said filler (E)comprises a fibrous, powdery or flaky filler.
 14. The method of claim 13wherein said filler comprises glass or carbon fiber.
 15. The method ofclaim 13 wherein said filler comprises a mixture of a fibrous fillerwith a powdery or flaky filler.
 16. A polyarylene sulfide resincomposition prepared by the method of claims 1 or
 2. 17. The polyarylenesulfide resin composition of claim 16 further including 1 to 400 partsby weight of a filler (E).
 18. The polyarylene sulfide resin compositionof claim 17 wherein said filler comprises a fibrous, powdery or flakyfiller.
 19. The polyarylene sulfide resin composition of claim 17wherein said filler (E) comprises glass or carbon fiber.
 20. Thepolyarylene sulfide resin composition of claim 16 wherein saidpolyarylene sulfide is selected from a homopolymer composed ofp-phenylene sulfide units or a copolymer composed of a mixture ofp-phenylene sulfide units and m-phenylene sulfide units.